Corneal diseases represent a significant global health challenge, often resulting in blindness, for which penetrating keratoplasty is the clinical gold standard. However, in cases involving compromised ocular surfaces or graft failure, osteo-odonto keratoprosthesis (OOKP) emerges as a vital yet costly and complex alternative. Thus, there is an urgent need to introduce soft biomaterials that mimic the corneal tissue, considering its translation’s physicochemical, biological, and economic costs. This study introduces a cross-linked mixture of economically viable biomaterials, including gelatin, chitosan, and poly-D-lysine, that mimic corneal properties. The physicochemical evaluation of certain mixtures, specifically gelatin, chitosan, and poly-D-lysine cross-linked with 0.10% glutaraldehyde, demonstrates that properties such as swelling, optical transmittance, and thermal degradation are comparable to those of native corneas. Additionally, constructs fabricated with poly-D-lysine exhibit good cytocompatibility with fibroblasts at 72 h. These findings suggest that low-cost biopolymers, particularly those incorporating poly-D-lysine, mimic specific corneal characteristics and have the potential to foster fibroblast survival. While further studies are required to reach a final corneal-mimicking solution, this study contributes to positioning low-cost reagents as possible alternatives to develop biomaterials with physicochemical properties like those of the human cornea.